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Vol. 17 (2025)

Transition Metal Carbonitride MXenes Anchored with Pt Sub-Nanometer Clusters to Achieve High-Performance Hydrogen Evolution Reaction at All pH Range

https://doi.org/10.1007/s40820-025-01654-y
Zhihao Lei
Global Innovative Center of Advanced Nanomaterials, College of Engineering, Science and Environment, University of Newcastle, Callaghan, NSW 2308, Australia
Sajjad Ali
Energy, Water, and Environment Lab, College of Humanities and Sciences, Prince Sultan University, 11586 Riyadh, Saudi Arabia
CI Sathish
Global Innovative Center of Advanced Nanomaterials, College of Engineering, Science and Environment, University of Newcastle, Callaghan, NSW 2308, Australia
MuhammadIbrar Ahmed
Global Innovative Center of Advanced Nanomaterials, College of Engineering, Science and Environment, University of Newcastle, Callaghan, NSW 2308, Australia
Jiangtao Qu
School of Physics, University of Sydney, Sydney, NSW 2000, Australia
Rongkun Zheng
School of Physics, University of Sydney, Sydney, NSW 2000, Australia
Shibo Xi
Institute of Chemical and Engineering Sciences, A*STAR , Singapore 627833, Singapore
Xiaojiang Yu
Singapore Synchrotron Light Source, National University of Singapore, Singapore 117603, Singapore
M. B. H. Breese
Singapore Synchrotron Light Source, National University of Singapore, Singapore 117603, Singapore
Chao Liu
Institute for Frontier Materials, Deakin University, Waurn Ponds, Victoria 3216, Australia
Jizhen Zhang
Guangdong Provincial Key Laboratory of Natural Rubber Processing, Agricultural Products Processing Research Institute, Chinese Academy of Tropical Agricultural Sciences, Zhanjiang 524001, People’s Republic of China
Shuai Qi
College of Chemistry Environmental Engineering, Shenzhen University, Shenzhen 518060, Guangdong, People’s Republic of China
Xinwei Guan
Global Innovative Center of Advanced Nanomaterials, College of Engineering, Science and Environment, University of Newcastle, Callaghan, NSW 2308, Australia
Vibin Perumalsamy
Global Innovative Center of Advanced Nanomaterials, College of Engineering, Science and Environment, University of Newcastle, Callaghan, NSW 2308, Australia
Mohammed Fawaz
Global Innovative Center of Advanced Nanomaterials, College of Engineering, Science and Environment, University of Newcastle, Callaghan, NSW 2308, Australia
Jae‑Hun Yang
Global Innovative Center of Advanced Nanomaterials, College of Engineering, Science and Environment, University of Newcastle, Callaghan, NSW 2308, Australia
Mohamed Bououdina
Global Innovative Center of Advanced Nanomaterials, College of Engineering, Science and Environment, University of Newcastle, Callaghan, NSW 2308, Australia
Kazunari Domen
Research Initiative for Supra-Materials Interdisciplinary Cluster for Cutting Edge Research, Shinshu University, 4‑17‑1, Wakasato, Nagano‑shi, Nagano 380‑8533, Japan
Ajayan Vinu
Global Innovative Center of Advanced Nanomaterials, College of Engineering, Science and Environment, University of Newcastle, Callaghan, NSW 2308, Australia
Liang Qiao
School of Physics, University of Electronic Science and Technology of China, Chengdu 610054, People’s Republic of China
Jiabao Yi
Department of Chemical Engineering and Interdisciplinary Research Center for Hydrogen Technologies and Carbon Management (IRC‑HTCM), King Fahd University of Petroleum and Minerals, 31261 Dhahran, Saudi Arabia

Corresponding Author: Jiabao Yi

Jiabao.yi@kfupm.edu.sa

Nano-Micro Letters, Vol. 17 (2025), Article Number: 123

Abstract

Transition metal carbides, known as MXenes, particularly Ti3C2Tx, have been extensively explored as promising materials for electrochemical reactions. However, transition metal carbonitride MXenes with high nitrogen content for electrochemical reactions are rarely reported. In this work, transition metal carbonitride MXenes incorporated with Pt-based electrocatalysts, ranging from single atoms to sub-nanometer dimensions, are explored for hydrogen evolution reaction (HER). The fabricated Pt clusters/MXene catalyst exhibits superior HER performance compared to the single-atom-incorporated MXene and commercial Pt/C catalyst in both acidic and alkaline electrolytes. The optimized sample shows low overpotentials of 28, 65, and 154 mV at a current densities of 10, 100, and 500 mA cm−2, a small Tafel slope of 29 mV dec−1, a high mass activity of 1203 mA mgPt−1 and an excellent turnover frequency of 6.1 s−1 in the acidic electrolyte. Density functional theory calculations indicate that this high performance can be attributed to the enhanced active sites, increased surface functional groups, faster charge transfer dynamics, and stronger electronic interaction between Pt and MXene, resulting in optimized hydrogen absorption/desorption toward better HER. This work demonstrates that MXenes with a high content of nitrogen may be promising candidates for various catalytic reactions by incorporating single atoms or clusters.


Highlights:
1 Two-dimensional mono- and few-layered Ti3CNTx MXene nanosheets with extremely high nitrogen content were synthesized.
2 Better performance for hydrogen evolution reaction (HER) than Pt/C catalyst in acidic, neutral and alkaline solutions.
3 Exceptional performance of HER in both acidic and alkaline solutions.
4 A large current density (> 500 mA cm−2) has been achieved for HER.

Keywords

MXene Hydrogen evolution reaction Single atom Two-dimensional nanosheets Density functional theory
Lei, Zhihao, Sajjad Ali, CI Sathish, MuhammadIbrar Ahmed, Jiangtao Qu, Rongkun Zheng, Shibo Xi, Xiaojiang Yu, M. B. H. Breese, Chao Liu, Jizhen Zhang, Shuai Qi, Xinwei Guan, Vibin Perumalsamy, Mohammed Fawaz, Jae‑Hun Yang, Mohamed Bououdina, Kazunari Domen, Ajayan Vinu, Liang Qiao, and Jiabao Yi. 2025. “Transition Metal Carbonitride MXenes Anchored With Pt Sub-Nanometer Clusters to Achieve High-Performance Hydrogen Evolution Reaction at All PH Range”. Nano-Micro Letters 17 (January):123. https://doi.org/10.1007/s40820-025-01654-y.
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